Many current technological applications are based on the electrical properties of materials. Among these, ferroelectricity, antiferroelectricity, paraelectricity, and resistivity are the most important to be studied and controlled. To overcome important drawbacks of sintered ceramics or single crystals with these characteristics, the preparation of glass-ceramics with these phases dispersed in a glass matrix is a possible solution. The formation of glass-ceramics shows great advantages—their properties (optical, electrical, mechanical, and chemical) can be controlled via the volume fraction of the dispersed active phase. Thus, the preparation and properties of glass-ceramics containing ferroelectric crystallites embedded in the glass matrix have received considerable interest. This article discusses state-of-the-art preparation of glass-ceramics with one important technological ferroelectric crystal, lithium niobate (LiNbO3). Since the preparation of LiNbO3 single crystals by traditional growth techniques is technically difficult and economically costly—and with dense ceramics, it is difficult to achieve a congruent composition—scientific research on the fabrication methods of inorganic glasses containing LiNbO3 crystallites is an important current topic.